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Marc Leonetti

Publications and source records attributed to Marc Leonetti.

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Non-contact mechanics of soft and liquid interfaces by hydrodynamic confinement using a frequency-modulated AFM

Measuring the mechanical response of liquid interfaces without direct contact remains a major experimental challenge, particularly in liquid-liquid systems where no solid reference exists. Here, we develop a frequency-modulation atomic force microscopy (FM-AFM) method that probes liquid interfaces through the hydrodynamic confinement of a viscous liquid film between an oscillating probe and the interface. This approach provides simultaneous access to the in-phase and dissipative components of the effective mechanical response under confinement. The method is first validated on a liquid-solid interface, where the measured confinement thickness and the evolution of the mechanical impedance are consistent with elastohydrodynamic theory over nearly one decade in elastic modulus. It is then applied to a liquid-liquid interface, which exhibits a predominantly viscous response with a finite in-phase contribution and a confinement thickness in the micrometric range. These results show that hydrodynamic confinement provides a sensitive, non-contact approach to compare the mechanical response of soft and liquid interfaces, and opens new perspectives for investigating complex and highly deformable systems such as polymer films, biological membranes, and rafts of nanoparticles.

cond-mat.soft

Deformation and orientation of a capsule with viscosity contrast in linear flows: a theoretical study

We develop a perturbation theory to study the shape and the orientation of an initially spherical capsule of radius R with a viscosity contrast, a surface tension {\sigma} and a bending rigidity $\kappa$ in linear flows. The elastic mechanical response of membrane to deformations is described by three elastic constitutive law which are either Hookean, Neohookean or Skalak type leading to the introduction of a surface shear elastic modulus $G_s$ and the Poisson ratio (or analog quantities). At the leading order, the deformation, i.e. the so-called Taylor parameter is proportional to the elastic capillary number Ca which evaluates the ratio between the external viscous stress and the elastic membrane response. In this linear regime, the results do not depend on the elastic constitutive law as expected. Without surface tension and bending rigidity, we recover the results of Barthes-Biesel & Rallison (1981) and notably the fact that the Taylor parameter does not depend on the viscosity contrast $\lambda$ contrary to the case of a viscous droplet. In our more general model, the deformation does no longer depend on $\lambda$ at the upper order. Now, the Taylor parameter also depends on two other dimensionless numbers: the surface elastocapillary ratio $\sigma/G_s$ and the dimensionless bending rigidity $B= \kappa/G_sR^2$. At the further order, the angle of inclination of the capsule with the direction of the shear flow, the analog of the Chaffey and Brenner equation for droplets is determined in each case. The results are in excellent agreement with the numerical ones performed with a code based on the boundary integral method providing an useful method to valid numerical developments.

cond-mat.soft

Early bloodmaterial interfacial events and capillary transport on nanoparticle modified nanofibers

Electrospun poly(\epsilon-caprolactone) (PCL)nanofibrous mats are widely considered for blood-contacting wound dressings and small-diameter vascular applications; however, their intrinsic hydrophobicity limits rapid wetting and controlled interaction with blood. In this work, we modulate the interfacial response of PCL nanofibers by incorporating oxide-shelled silicon nanoparticles (SiNPs) synthesized by pulsed laser ablation in liquid, a ligand-free approach that avoids organic stabilizers and preserves surface reactivity. Two composite architectures were designed: SiNPs embedded within the fiber bulk (PAC1,4,16) and SiNPs preferentially exposed at the fiber surface (SPAC1,4,16), with systematically increasing nanoparticle loadings. Structural characterization confirmed the retention of a homogeneous fibrous morphology and the targeted nanoparticle distribution. The dynamic interaction with whole blood was quantified using time-resolved contact-angle measurements, complemented by top-view optical microscopy and three-dimensional profilometry of dried droplets. Pristine PCL remained strongly hydrophobic whereas a hydrophilic PCL functionalized with APTES showed rapid spreading. Incorporation of SiNPs within the fiber volume led to only a moderate enhancement of wettability, and dried droplets retained compact morphologies with limited spreading. In contrast, surface-decorated mats displayed a sharp, concentration-dependent transition toward highly wettable behavior: for SPAC16, the contact angle fell below 20, droplet profiles became markedly flattened, and microscopy revealed extended plasma-rich regions surrounding a red-cell-rich core, indicative of pronounced phase separation within the nanofibrous network.

cond-mat.soft

Drop deformation with soluble surfactants in linear flows: role of adsorption-desorption

Drop deformation in shear flow is determined up to second order theory in Ca while considering kinetic effects on surfactants distributions in steady state. Surfactants inside the drop are adsorbed faster than those on the surface leading to an increase in total surfactants concentration on the semi-minor axis of the ellipsoidal droplet. New expressions for Taylor deformation and angle deviation are proposed involving kinetics effects. Theoretical calculations lead to a possibility of lesser deformation than the usual limit condition and a minor correction for the deviation angle.

cond-mat.soft

Margination of artificially stiffened red blood cells

Margination, a fundamental process in which leukocytes migrate from the flowing blood to the vessel wall, is well-documented in physiology. However, it is still an open question on how the differences in cell size and stiffness of white and red cells contribute to this phenomenon. To investigate the specific influence of cell stiffness, we conduct experimental and numerical studies on the segregation of a binary mixture of artificially stiffened red blood cells within a suspension of healthy cells. The resulting distribution of stiffened cells within the channel is found to depend on the channel geometry, as demonstrated with slit, rectangular, and cylindrical cross-sections. Notably, an unexpected central peak in the distribution of stiffened RBCs, accompanied by fourfold peaks at the corners, emerges in agreement with simulations. Our results unveil a non-monotonic variation in segregation/margination concerning hematocrit and flow rate, challenging the prevailing belief that higher flow rates lead to enhanced margination.

cond-mat.soft

Structural characterization of the interfacial self-assembly of chitosan with oppositely charged surfactant

Controlling the assembly of polyelectrolytes and surfactant at liquid-liquid interfaces offers new ways to fabricate soft materials with specific physical properties. However, little is known of the relationships between the kinetics of interfacial assembly, structural and rheological properties of such interfaces. We studied the kinetics at water-oil interface of the assembly of a positively charged biopolymer, chitosan, with an anionic fatty acid using a multi-scale approach. The growth kinetics of the membrane was followed by interfacial rheometry and space- and time- resolved dynamic light scattering. This set of techniques revealed that the interfacial complexation was a multi-step process. At short time-scale, the interface was fluid and made of heterogeneous patches. At a 'gelation' time, the surface elastic modulus and the correlation between speckles increased sharply meaning that the patches percolated. Confocal and electron microscopy confirmed this picture, and revealed that the basic brick of the membrane was sub-micrometric aggregates of chitosan / fatty acid.

cond-mat.soft

Membrane emulsification for the production of suspensions of uniform microcapsules with tunable mechanical properties

A way forward for high throughput fabrication of microcapsules with uniform size and mechanical properties was reported irrespective of the kinetic process of shell assembly. Microcapsules were produced using lab-scale emulsification equipment with a micro-engineered membrane in the size range 10-100 $\mu$m. The shell of the microcapsules was assembled at the water-oil interface by complexation of polyelectrolytes or cross-linking of proteins providing two different kinetic processes. Elasticity of microcapsules was characterized with an automated extensional flow chamber. Process parameters were optimized to obtain suspensions with size variations of 15%. Some strategies were developed to obtain uniform elastic properties according to the kinetics of shell assembly. If kinetics is limited by diffusion, membrane emulsification and shell assembly have to be split into two steps. If kinetics is limited by the quantity of reactants encapsulated in the droplet, variations of elastic properties result only from size variations.

cond-mat.soft

Effect of pulse width on the dynamics of a deflated vesicle in unipolar and bipolar pulsed electric fields

Giant unilamellar vesicles subjected to pulsed direct-current (pulsed-DC) fields are promising biomimetic systems to investigate the electroporation of cells. In strong electric fields, vesicles undergo significant deformation, which strongly alters the transmembrane potential, consequently the electroporation. Previous theoretical studies investigated the electrodeformation of vesicles in DC fields (which are not pulsed). In this work, we computationally investigate the deformation of a deflated vesicle under unipolar, bipolar, and two-step unipolar pulses and show sensitive dependence of intermediate shapes on type of pulse and the pulse width. Starting with the stress-free initial shape of a deflated vesicle, which is similar to a prolate spheroid, the analysis is presented for the cases with higher and lower conductivities of the inner fluid medium relative to the outer fluid medium. For the ratio of inner to outer fluid conductivity, $\sigma_\mathrm{r}$ = 10, the shape always remains prolate, including when the field is turned off. For $\sigma_\mathrm{r} = 0.1$, several complex dynamics are observed, such as the prolate-to-oblate (PO), prolate-to-oblate-to-prolate (POP) shape transitions in time depending upon the strength of the field and the pulse properties. In this case, on turning off the field, a metastable oblate equilibrium shape is seen, that seems to be a characteristics of a deflated vesicle leading to POPO transitions. When a two-step unipolar pulse (a combination of a strong and a weak subpulse) is applied, a vesicle can reach an oblate or a prolate final shape depending upon the relative durations of the two subpulses.

cond-mat.soft

Oblate to prolate transition of a vesicle in shear flow

Vesicles are micrometric soft particles whose the membrane is a two-dimensional incompressible fluid governed by bending resistance leading to a zoology of shapes. The dynamics of deflated vesicles in shear flow with a bottom wall, a first minimal configuration to consider confined vesicles is investigated using numerical simulations. Coexistence under flow of oblate (metastable) and prolate (stable) shapes is studied in details. In particular, we discuss the boundaries of the region of coexistence in the (v, Ca) plane where v is the reduced volume of the vesicle and Ca the Capillary number. We characterize the transition from oblate to prolate and analyse the divergence of the transition time near the critical capillary number. We then analyse lift dynamics of oblate vesicle in the weak flow regime.

cond-mat.soft

Dynamics of Particle Migration in Confined ViscoElastic Poiseuille Flows

Particles migrate in the transverse direction of the flow due to the existence of normal stress anisotropy in weakly viscoelastic liquids. We test the ability of theoretical predictions to predict the transverse velocity migration of particles in a confined Poiseuille flow according to the viscoelastic constitutive parameters of dilute polymers solutions. Firstly, we carefully characterize the viscoelastic properties of two families of dilute polymer solutions at various concentrations using shear rheometry and capillary breakup experiments. Secondly, we develop a specific 3D particle tracking velocimetry method to measure with a high accuracy the dynamics of particles focusing in flow for Weissenberg numbers Wi ranging from $10^{-2}$ to $10^{-1}$ and particle confinement $\beta$ of 0.1 and 0.2. The results show unambiguously that the migration velocity scales as $\text{Wi}\beta^2$, as expected theoretically for weakly elastic flows of an Oldroyd-B liquid. We conclude that classic constitutive viscoelastic laws are relevant to predict particle migration in dilute polymer solutions whereas detailed analysis of our results reveals that theoretical models overestimate by a few tenth the efficiency of particle focusing.

physics.flu-dyn